Trends in background levels of persistent organic pollutants at Kosetice observatory, Czech Republic. Part I. Ambient air and wet deposition 1996–2005w Ivan Holoubek, abc Jana Kla´nova´,* ac Jirˇ ı´ Jarkovsky´ a and Jirˇı´ Kohoutek ac Received 17th January 2007, Accepted 8th May 2007 First published as an Advance Article on the web 21st May 2007 DOI: 10.1039/b700750g Kosetice observatory is a facility of the Czech Hydrometeorological Institute, which is a part of the European Monitoring and Evaluation Programme (EMEP) network. Persistent organic pollutants (POPs: PCBs, DDTs, HCHs, PAHs) have been monitored in all environmental matrices using the integrated monitoring approach. Generally, the atmospheric levels of POPs in this Central European background station (mean values: 0.115 ng m 3 for P PCBs, 0.040 ng m 3 for P DDTs, 0.077 ng m 3 for P HCHs, and 17 ng m 3 for P PAHs) are significantly higher than those in other EMEP stations localized mostly in Northern and Western Europe. Long-term trends of POP concentrations in the ambient air and wet deposition are presented in this article and they show a slow decline in the last decade for most of the investigated compounds. Temporally increased levels of certain chemicals were associated with some local climatic (floods) or socio-economic (fuel prices) factors. Introduction A risk of irreversible changes in the terrestrial and aquatic ecosystems as well as a danger of the global climate change caused by environmental pollution was first recognized in the early 1960s. However, detection of such changes in the natural environment at regional and global levels requires a coordi- nated monitoring effort based on broad international coopera- tion. First, international monitoring programs were introduced in the 1960s and 1970s by the international institu- tions (WMO, ECE, UNEP), and they focused on various environmental aspects, including effects of human activities on climate change, trans-boundary transport of pollutants and exchange of chemicals between environmental compartments. Persistent organic pollutants (POPs), as the substances prone to long-range atmospheric transport and deposition in distant regions, 1,2 are the compounds of such concern. Their global impact has been apparent since the members of this group were detected in polar regions at levels posing risks to both wildlife 3 and humans. 4 In 1992, a newly established initiative of the United Nations Economic Commission for Europe (UN-ECE) had prepared a protocol on POPs 2 with the goal to control, reduce or elim- inate their discharge, emission and release. A similar program of the United Nations Environment Program was introduced in cooperation with the International Forum for Chemical Safety (UNEP/IFCS). 5 It has been recognized that an impor- tant step in establishment of effective control measures is the inventory of current POP concentrations in various environ- mental compartments, and assessment of their time trends. Determination of POP concentrations in the atmosphere, wet and dry deposition, surface water, sediment, soil and vegeta- tion is desirable under various geographic and climatic condi- tions. Such information improves our understanding of the pathways and potential effects of chemical substances, and defines specific parameters for exposure assessment. At the same time, new data sets valuable for validation of regional and global models of atmospheric transport and environmen- tal fate are generated. The number of sites where POPs are continuously monitored over extended time periods in several environmental compartments is, however, very limited. One of the programs coordinating such a monitoring effort on multiple sites is the European Monitoring and Evaluation Programme (EMEP). It was established with the main goal of providing the governments and subsidiary bodies under the Convention on Long Range Trans-boundary Air Pollution with qualified scientific information supporting development and evaluation of the international protocols. The EMEP program was initially focused on the trans-boundary transport of acidification and eutrophication. Later, its scope broadened to address a formation of surface ozone, and more recently it also covers volatile organic compounds, persistent organic pollutants, and heavy metals. A map of the EMEP stations (including analyzed matrices) is presented in Fig. 1. 6 Only six (out of fifteen) EMEP sites reported POPs in both air and wet deposition in 2004. Kosetice station (furthest to the right in Fig 1) was the only site where POPs were also a RECETOX, Faculty of Science, Masaryk University, Kamenice 126/ 3, 625 00 Brno, Czech Republic. E-mail: [email protected]; Fax: +420 549492840; Tel: +420 549495149 b TOCOEN, s.r.o., Kamenice 126/3, 625 00 Brno, Czech Republic, E-mail: [email protected]; Fax: +420 549492840; Tel: +420 549495149 c National POPs Centre of the Czech Republic, Kamenice 126/3, 625 00 Brno, Czech Republic. E-mail: [email protected]; Fax: +420 549492840; Tel: +420 549495149 w Presented at Sources, Fate, Behaviour and Effects of Organic Chemicals at the Regional and Global Scale, 24th–26th October 2006, Lancaster, UK. This journal is c The Royal Society of Chemistry 2007 J. Environ. Monit., 2007, 9, 557–563 | 557 PAPER www.rsc.org/jem | Journal of Environmental Monitoring
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Trends in background levels of persistent organic pollutants at Kosetice
observatory, Czech Republic.
Part I. Ambient air and wet deposition 1996–2005w
Ivan Holoubek,abc
Jana Klanova,*ac
Jirı Jarkovskyaand Jirı Kohoutek
ac
Received 17th January 2007, Accepted 8th May 2007
First published as an Advance Article on the web 21st May 2007
DOI: 10.1039/b700750g
Kosetice observatory is a facility of the Czech Hydrometeorological Institute, which is a part of
the European Monitoring and Evaluation Programme (EMEP) network. Persistent organic
pollutants (POPs: PCBs, DDTs, HCHs, PAHs) have been monitored in all environmental
matrices using the integrated monitoring approach. Generally, the atmospheric levels of POPs in
this Central European background station (mean values: 0.115 ng m�3 forP
PCBs, 0.040 ng m�3
forP
DDTs, 0.077 ng m�3 forP
HCHs, and 17 ng m�3 forP
PAHs) are significantly higher
than those in other EMEP stations localized mostly in Northern and Western Europe. Long-term
trends of POP concentrations in the ambient air and wet deposition are presented in this article
and they show a slow decline in the last decade for most of the investigated compounds.
Temporally increased levels of certain chemicals were associated with some local climatic (floods)
or socio-economic (fuel prices) factors.
Introduction
A risk of irreversible changes in the terrestrial and aquatic
ecosystems as well as a danger of the global climate change
caused by environmental pollution was first recognized in the
early 1960s. However, detection of such changes in the natural
environment at regional and global levels requires a coordi-
nated monitoring effort based on broad international coopera-
tion. First, international monitoring programs were
introduced in the 1960s and 1970s by the international institu-
tions (WMO, ECE, UNEP), and they focused on various
environmental aspects, including effects of human activities
on climate change, trans-boundary transport of pollutants and
exchange of chemicals between environmental compartments.
Persistent organic pollutants (POPs), as the substances prone
to long-range atmospheric transport and deposition in distant
regions,1,2 are the compounds of such concern. Their global
impact has been apparent since the members of this group
were detected in polar regions at levels posing risks to both
wildlife3 and humans.4
In 1992, a newly established initiative of the United Nations
Economic Commission for Europe (UN-ECE) had prepared a
protocol on POPs2 with the goal to control, reduce or elim-
inate their discharge, emission and release. A similar program
of the United Nations Environment Program was introduced
in cooperation with the International Forum for Chemical
Safety (UNEP/IFCS).5 It has been recognized that an impor-
tant step in establishment of effective control measures is the
inventory of current POP concentrations in various environ-
mental compartments, and assessment of their time trends.
Determination of POP concentrations in the atmosphere, wet
and dry deposition, surface water, sediment, soil and vegeta-
tion is desirable under various geographic and climatic condi-
tions. Such information improves our understanding of the
pathways and potential effects of chemical substances, and
defines specific parameters for exposure assessment. At the
same time, new data sets valuable for validation of regional
and global models of atmospheric transport and environmen-
tal fate are generated. The number of sites where POPs are
continuously monitored over extended time periods in several
environmental compartments is, however, very limited.
One of the programs coordinating such a monitoring effort
on multiple sites is the European Monitoring and Evaluation
Programme (EMEP). It was established with the main goal of
providing the governments and subsidiary bodies under the
Convention on Long Range Trans-boundary Air Pollution
with qualified scientific information supporting development
and evaluation of the international protocols. The EMEP
program was initially focused on the trans-boundary transport
of acidification and eutrophication. Later, its scope broadened
to address a formation of surface ozone, and more recently it
also covers volatile organic compounds, persistent organic
pollutants, and heavy metals. A map of the EMEP stations
(including analyzed matrices) is presented in Fig. 1.6
Only six (out of fifteen) EMEP sites reported POPs in both
air and wet deposition in 2004. Kosetice station (furthest to
the right in Fig 1) was the only site where POPs were also
cNational POPs Centre of the Czech Republic, Kamenice 126/3, 62500 Brno, Czech Republic. E-mail: [email protected]; Fax:+420 549492840; Tel: +420 549495149w Presented at Sources, Fate, Behaviour and Effects of OrganicChemicals at the Regional and Global Scale, 24th–26th October2006, Lancaster, UK.
This journal is �c The Royal Society of Chemistry 2007 J. Environ. Monit., 2007, 9, 557–563 | 557
PAPER www.rsc.org/jem | Journal of Environmental Monitoring
determined in other environmental matrices. Kosetice obser-
vatory of the Czech Hydrometeorological Institute is located
in the southern Czech Republic (N491350; E151050). The
climatic classification of the region is a moderately warm
and moderately humid upland zone with a mean annual
temperature of 7.1 1C, mean annual total precipitation of
621 mm, between 60 and 100 days with snow-cover per year,
1800 hours of sunshine per year, and prevailing westerly
winds. The observatory was established as a regional station
of an integrated background monitoring network in the late
1970s.
All measurements assigned to EMEP stations (including
VOCs, POPs and heavy metals) are currently implemented in
Kosetice,7–13 and monitoring design is based on the EMEP
POP monitoring strategy.14 Samples of the ambient air, wet
deposition, surface water, sediment, soil and biota, as the key
components of the environmental system, are collected. The
ecosystem indicators are further applied to determine the
current state, anthropogenic impacts and influences, and to
predict the future changes of terrestrial and freshwater eco-
systems in a long-term perspective.14 A dataset generated over
ten years of integrated monitoring in Kosetice was used in this
study to assess the Central European trends in background
levels of persistent organic pollutants.
Methods and materials
Selection of compounds and matrices
16 US EPA polycyclic aromatic hydrocarbons (PAHs), 7
a BQL = below quantification limit. Quantification limit is 1 pg m�3
for the individual compounds in the ambient air, and 50 pg L�1 in the
rain water.
This journal is �c The Royal Society of Chemistry 2007 J. Environ. Monit., 2007, 9, 557–563 | 559
well pronounced as it is in the case of PAHs, it can still be
detected for PCBs in Fig. 3, and for pesticides in Fig. 4 and 5.
POP concentrations in wet deposition reflect the air con-
centrations. Phenanthrene, fluorene, and pyrene were the most
abundant compounds in all wet deposition samples; g-HCH
was detected in the highest concentrations of all chlorinated
compounds. While the mean concentration of PAHs (EPA 16)
was 120 ng L�1, the mean concentrations of chlorinated
compounds were lower: 0.5 ng L�1 for the sum of 7 PCBs, 5
ng L�1 for the sum of HCHs, 0.2 ng L�1 for the sum of DDT,
DDD, and DDE, and 0.05 ng L�1 for HCB. A seasonality in
the PAH rain water concentrations similar to the atmospheric
concentrations can be seen in Fig. 6.
While the minimum summer concentration was only 2 ng
L�1, the maximum winter concentration reached as high as
6310 ng L�1.
The annual median concentrations were calculated for all
POP subgroups (PAHs, PCBs, DDTs, HCHs and HCB) in the
air and wet deposition, and the resulting ten annual values for
the period of 1996–2005 were compared to evaluate the long-
term trends for each group of compounds and each matrix
(Fig. 7 and 8). The analysis revealed time related changes in
the amounts of chemical species. An interesting time develop-
ment can be seen for the sum of 16 PAHs in the atmospheric
gas phase (Fig. 7): a very pronounced decrease between 1996
and 2000 was followed by an increase in 2001–2002. This effect
probably reflects the local economic situation in the Czech
Republic where growing prices of gas in 2001 brought back the
coal and wood combustion in local heating systems. A similar
trend can be identified for the particulate phase as well as the
wet deposition. In the case of wet deposition, the annual
medians of PAH concentrations do not show any increase in
2001 (Fig. 8), however, elevated winter maxima can be identi-
fied in 2002 (Fig. 6).
The annual medians of PCBs also indicate a general de-
creasing trend interrupted by two periods of higher concentra-
tions (Fig. 7): 1997–1998 and 2000–2001. As can be seen from
Fig. 3, there are significantly elevated summer maxima of PCB
concentrations in 1997 and 1998 (maxima 390 pg m�3 and 337
pg m�3 for the sum of 7 PCB congeners in 1997 and 1998,
respectively). In contrast, summer maxima between 2000 and
2001 were lower (167 pg m�3 and 246 pg m�3) but due to the
higher winter minima (52 pg m�3—same as in 1998), the
annual medians remained quite high. Interestingly, in the
2000–2001 period there was also a significant fraction of
particle associated PCBs (Fig. 3). In contrast, high summer
maxima were observed in 2002 and 2003 (366 pg m�3 for the
sum of 7 congeners) but due to the low winter levels, it was not
reflected in the annual medians. These fluctuations in the
annual medians of PCBs may reflect the major flood events
in the Czech Republic in 1997 and 2002. A large area of central
and southern Moravia (to the east from Kosetice) was flooded
in 1997, including industrial and agricultural facilities where
various chemicals were stored. The floods were followed by
extremely hot summer, therefore those chemicals could eva-
porate from impacted areas and be a subject of atmospheric
transport. Similarly, the central part of Bohemia (to the west
from Kosetice, Prague included) was flooded in 2002. Several
large chemical enterprises located to the north of Prague were
severely damaged, and a variety of chemicals escaped to the
surface waters and was distributed with the flood. According
Fig. 2P
PAHs in the ambient air, Kosetice observatory, 1996–2005.
Fig. 3P
PCBs in the ambient air, Kosetice observatory, 1996–2005.
Fig. 4P
HCHs in the ambient air, Kosetice observatory, 1996–2005.
Fig. 5P
DDTs in the ambient air, Kosetice observatory, 1996–2005.
560 | J. Environ. Monit., 2007, 9, 557–563 This journal is �c The Royal Society of Chemistry 2007
to the results of our previous research, which focused on the
impact of these flood events on aquatic and terrestrial envir-
onments,20 one of the effects of floods is a re-distribution of
the old burdens from the river sediments to the surface layers
of the soils that were flooded. Semi-volatile persistent organic
compounds can easily re-evaporate from these top soil levels
during the warm season. This is probably the source of
elevated atmospheric concentration of chlorinated POPs in
the years following these disasters. The reason why the floods
in 1997 so significantly affected the background levels of
PCBs, and the flood events in 2002 had a much smaller impact,
can be a character of the flooded regions. In 1997, the region
with highest PCB levels in environmental matrices (including
mother milk) in the Czech Republic was impacted. A paint
factory located in this area (Colorlak) was the major consumer
of PCB mixtures produced in the former Czechoslovakia
(Chemko Strazske)21 under the commercial name Delor, and
PCB-containing paints were heavily used in this region.
The same reasoning can be applied to explain the elevated
levels of organochlorine pesticides over the same periods (Fig.
4 and 5). HCHs exhibited extremely high levels in the summer
of 1998, and gradually decreased in 1999 and 2000 (Fig. 4 and
7). An elevated fraction of b-HCH was observed in 1999 and
2000 (Fig. 4) suggesting that some old deposits of HCH
technical mixtures or ballast HCH congeners were newly
exposed. The levels have been stabilizing since 2001, showing
only a typical seasonal variability.
DDTs followed the same pattern with very high summer
maxima in 1997 and 1998 and a gradual decrease until 2001
(Fig. 5 and 7). However, since the second increase in
2002–2003, the concentrations of DDT and its metabolites
have stabilized at elevated levels. This is probably again
connected to the flood events in 2002, when the chemical
factories which earlier produced pesticides, agricultural enter-
prises and pesticide storage facilities were affected and large
amounts of pesticides escaped to the environment. However,
the influence of the local sources (evaporation from the soils or
ponds) cannot be excluded. A new DDT fingerprint is typical
with a less pronounced seasonal variability and the enhanced
fraction of p,p0-DDD.
HCB is the only analyte which shows a statistically signifi-
cant increasing trend in its air concentrations. We can still
detect high summer air concentrations of HCB following the
floods in 1997 but—similarly to DDT—the floods in 2002
seem to have had a more lasting impact. The very high
Fig. 6P
PAHs in rain (monthly means), Kosetice observatory,
1996–2005.
Fig. 7 Temporal trends of POPs in the air, gas phase. The line
represents a linear trend estimate.
Fig. 8 Time related trends of POPs in the wet deposition. The line
represents an estimated trend.
This journal is �c The Royal Society of Chemistry 2007 J. Environ. Monit., 2007, 9, 557–563 | 561
concentrations from 2002 and 2003 have only declined very
slowly in the next few years. Thus, what seems to be an
increasing trend in the statistical analysis of annual medians
is most probably only a very slow recovery of the ecosystem
from the severe impact of the natural disaster. At the same
time, an extreme level of pentachlorobenzene as a degradation
product of HCB was detected in 2002.
Between 1987 and 2004, there have been ten reports pub-
lished by EMEP presenting data on POPs and heavy metals
from national and international monitoring programs.6,22,23
POPs were included in the EMEP’s monitoring program in
1999; however, data for POPs have been reported only from
countries around the North and Baltic Seas, in the Arctic and
from the Czech Republic. In general the concentrations de-
crease from south to north, except for a-HCH where the
highest concentration was seen in 2004 in Svalbard, Norway
(Zeppelin, 17 pg m�3) and Finland (Pallas, 18 pg m�3),
followed by lower concentrations in Sweden (Rao, 13 pg
m�3), Czech Republic (Kosetice, 12 pg m�3) and Iceland
(Storhovdi, 5 pg m�3).6 The presence of HCH in environments
far away from the sources is due to long-range atmospheric
transport. Preferential deposition and accumulation in polar
latitudes are expected according to the hypothesis of global
fractionation and cold condensation.24 Iceland, on the other
hand, is influenced by westerly air masses, which may explain
the lower concentrations. A similar monitoring study per-
formed in the Great Lakes area (Integrated Atmospheric
Deposition Network—IADN)25 found the a-HCH concentra-
tion in Chicago area (Lake Michigan, 45 pg m�3) lower than
the one in Eagle Harbor (Lake Superior, 52 pg m�3).
Concentrations of other POPs are much higher in the Czech
Republic than those observed in the Nordic countries. For
PCBs it is explained by the high historical usage in central
Europe26 and production of PCBs in the former Czechoslo-
vakia in significant amounts until 1984.21 The concentration
of, for instance, PCB 101 in Kosetice was 7 pg m�3 in 2004,
while it is only 1–2 pg m�3 in all the other stations. In the
Great Lakes area, for comparison, a concentration of
33 pg m�3 was measured for PCB 101 in Chicago, while it
was only 2 pg m�3 in Eagle Harbor.25
A similar situation was observed for DDTs. A DDE con-
centration as high as 21 pg m�3 was observed in Kosetice,
while it was only 3 pg m�3 in Sweden, 1 pg m�3 in Finland and
Svalbard, and below the detection limit in Iceland. The IADN
program reported 20 pg m�3 of DDE in Chicago and 1 pg m�3
in Eagle Harbor.25
Determination of PAHs in the air samples showed the levels
of 5.9 ng m�3 for phenanthrene and 279 pg m�3 for benzo(a)-
pyrene in Kosetice, 1.1 ng m�3 and 29 pg m�3 in Sweden, 470
pg m�3 and 33 pg m�3 in Finland, and 7 pg m�3 and 3 pg m�3
in Svalbard. At the Great Lakes, a concentration of 27.8 ng
m�3 was measured for phenanthrene and 230 pg m�3 for
benzo(a)pyrene in Chicago, while it was only 480 pg m�3 and
less than 1 pg m�3 in Eagle Harbor.25
A significant effort connected to the long-term ambient air
monitoring program in the Kosetice observatory is also fo-
cused on source identification. Due to the prevailing westerly
wind direction and the main sector of incoming air masses
between 2201 and 3201, major industrial and urban centers in
the Czech Republic, i.e. Prague, Plzen, and Ceske Budejovice
may act as source areas for Kosetice observatory. These
sources, of course, only contributed towards the end of air
parcels’ traveling to the site. A detailed analysis of the wind
trajectories and the origin of air masses is needed in order to
identify other, more remote sources, and the main contribu-
tors to the atmospheric pollution at the background station.
Those tasks are currently being addressed.
Conclusions
Data from ten years of integrated monitoring at Kosetice
observatory were used in this project to assess long-term
trends of POPs in the ambient air and wet deposition in the
European continental background. Most of the selected com-
pounds exhibited decreasing trends in the last decade. This is
consistent with data reported from other European sites.6
The results of our project demonstrated that the long-term
background monitoring is not only an excellent way to study
the regional levels and trends, but also a powerful tool for
evaluation of the impact of various local and regional
events—from industrial accidents to natural disasters. As
such, this approach has the potential to play a crucial role in
the implementation of regional and global measures and
conventions on persistent toxic substances.
Monitoring data from Kosetice are currently being used for
the assessments of the sources and distribution processes, and
for the validation of long-range transport and environmental
fate models. This study was carried out as a contribution to
the ongoing national POPs inventory in the Czech Republic.
Acknowledgements
The project was supported by the Czech Hydrometeorological
Institute and the Czech Ministry of Education, Youth and
Sport (MSM 0021622412). The authors express their gratitude
to all colleagues from the Czech Hydrometeorological Insti-
tute and Masaryk University who participated in the sample
collection and analysis over the whole period of the project.
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